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钴替代减缓了低水超临界二氧化碳中镁橄榄石的碳酸化作用。

Cobalt substitution slows forsterite carbonation in low-water supercritical carbon dioxide.

作者信息

Loring John S, Webb Tenley E, Bowden Mark E, Engelhard Mark H, Kerisit Sebastien N

机构信息

Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, USA.

Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA 99354, USA.

出版信息

Phys Chem Chem Phys. 2024 Oct 23;26(41):26465-26471. doi: 10.1039/d4cp02092h.

Abstract

Cobalt recovery from low-grade mafic and ultramafic ores could be economically viable if combined with CO storage under low-water conditions, but the impact of Co on metal silicate carbonation and the fate of Co during the carbonation reaction must be understood. In this study, infrared spectroscopy was used to investigate the carbonation of Co-doped forsterite ((Mg,Co)SiO) in thin water films in humidified supercritical CO at 50 °C and 90 bar. Rates of carbonation of Co-doped forsterite to Co-rich magnesite ((Mg,Co)CO) increased with water film thickness but were at least 10 times smaller than previously measured for pure forsterite at similar conditions. We suggest that the smaller rates are due to thermodynamic drivers that cause water films on Co-doped forsterite to be much less oversaturated with respect to Co-doped magnesite, compared to the pure minerals.

摘要

如果能在低水条件下与碳储存相结合,从低品位镁铁质和超镁铁质矿石中回收钴在经济上可能是可行的,但必须了解钴对金属硅酸盐碳酸化的影响以及钴在碳酸化反应中的去向。在本研究中,利用红外光谱研究了在50°C和90巴的加湿超临界CO₂中,钴掺杂镁橄榄石((Mg,Co)SiO₄)在薄水膜中的碳酸化情况。钴掺杂镁橄榄石碳酸化为富钴菱镁矿((Mg,Co)CO₃)的速率随水膜厚度增加而增加,但至少比之前在类似条件下测量的纯镁橄榄石的速率小10倍。我们认为,速率较小是由于热力学驱动因素导致,与纯矿物相比,钴掺杂镁橄榄石上的水膜相对于钴掺杂菱镁矿的过饱和度要小得多。

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